Ruthenium Complexes of 2,2′-Bipyridine-6,6′-diphosphonate Ligands for Water Oxidation

被引:19
|
作者
Kamdar, Jayneil M. [1 ]
Marelius, David C. [1 ]
Moore, Curtis E. [2 ]
Rheingold, Arnold L. [2 ]
Smith, Diane K. [1 ]
Grotjahn, Douglas B. [1 ]
机构
[1] San Diego State Univ, Dept Chem & Biochem, 5500 Campanile Dr, San Diego, CA 92182 USA
[2] Univ Calif San Diego, Dept Chem & Biochem, 9500 Gilman Dr, La Jolla, CA 92093 USA
关键词
catalysis; phosphonate; redox chemistry; ruthenium; water splitting; METAL PHOSPHONATE CHEMISTRY; ARTIFICIAL PHOTOSYNTHESIS; BIPYRIDINE LIGANDS; SOLAR-ENERGY; CATALYST; INTERMEDIATE; PATHWAYS; BEHAVIOR; FAMILY; DIMER;
D O I
10.1002/cctc.201600359
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Two novel ruthenium complexes, [Ru(2,2'-bipyridine-6,6'-diphosphonato)(pic)(2)] (2) (pic = 4-picoline) and [Ru(6,6'-diisopropyl-2,2'-bipyridine-6,6'-diphosphonato)(pic)(2)] (3) bearing phosphonate groups have been synthesized and characterized by NMR spectroscopy, elemental analyses, X-ray crystallography, cyclic voltammetry, and UV/Vis spectroscopy. Both complexes show catalytic water oxidation activity by electrochemistry. At pH 7, the Ru-II/III redox couple of 2 is observed at a lower potential than that of 3, yet significantly, 3 oxidizes water at a lower onset potential. At pH1 however, 2 and 3 have comparable catalytic reactivity using sacrificial oxidant Ce-IV. We propose that water oxidation activities of 2 and 3 are influenced by overall charges. For example, in oxidizing from Ru-II to Ru-III at pH 7, 2 acquires a -1 overall charge whereas 3 acquires a +1 charge. Charge-dictated electrostatic effects may govern binding of a water molecule to the metal site.
引用
收藏
页码:3045 / 3049
页数:5
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